Publications

The authors have synthesized and characterized two novel Sr compounds: [Sr({mu}-ONc){sub 2}(HONc){sub 4}]{sub 2} (1, ONc = O{sub 2}CCH{sub 2}CMe{sub 3}), and Sr{sub 5}({mu}{sub 4}-O)({mu}{sub 3}-ONep){sub 4}({mu}-ONep){sub 4}(HONep)(solv){sub 4} [ONep = OCH{sub 2}CMe{sub 3}, solv = tetrahydrofuran (THF), 2a; 1-methyl-imidazole (MeIm), (2b)], that demonstrate increased solubility in comparison to the commercially available Sr precursors. The two metal centers of 1 share 4 unidentate bridging {mu}-ONc ligands and complete their octahedral geometry through the coordination of 4 monodentate terminal HONc ligands. The structure arrangement of the central core of 2a and b are identical, wherein 4 octahedral Sr atoms are arranged in a square geometry around a {mu}{sub 4}-O ligand. An additional 7-coordinated Sr atom sits directly atop the {mu}{sub 4}-O to form a square base pyramidal arrangement of the Sr atoms but the apical Sr-O distance is too long to be considered a bond. In solution, compound 1 is disrupted forming a monomer but 2a and b retain their structures.

Plate impact, shock wave experiments provide a unique method to investigate the time-dependent mechanisms and the kinetics associated with pressure-induced phenomena, such as chemical reactions and phase transformations. The very rapid and well defined loading conditions associated with plate-impact experiments permit real-time examination of the shock-induced changes. Further, the ability to propagate the shock wave along various crystallographic directions provides the means to perform careful analysis of the stress and orientational dependence. Recently, an experimental method has been developed to observe real-time changes in the absorption transmission of materials, with 100 or 200 ps resolution, in single-event, plate impact shock experiments [1-4]. These data can provide useful information regarding the material under investigation. In particular, the dependence of the absorption edge on photon energy can distinguish between direct and indirect electronic transitions, and can provide an estimate of the band-gap energy of the material [5]. Along with ab-initio techniques to calculate the electronic structure of a crystalline system, this electronic information can be used to gain insight regarding the crystal structure. As described in Ref. [1,2,4] the wurtzite-to-rocksalt phase transition in cadmium sulfide (CdS) is well suited to investigation through the use of fast electronic spectroscopy; the wurtzite and rocksalt phases exhibit a direct and indirect band gap with band gap energies of 2.5 and 1.5-1.7 eV, respectively [6-8]. The intent of this work was to use picosecond electronic spectroscopy and ab-initio methods to examine the real-time structural changes that occur in the initial stages of the shock-induced wurtzite-to-rocksalt phase transition in single crystal CdS.

Recently there has been a noted worldwide increase in violent actions including attempted sabotage at nuclear power plants. Several organizations, such as the International Atomic Energy Agency and the US Nuclear Regulatory Commission, have guidelines, recommendations, and formal threat- and risk-assessment processes for the protection of nuclear assets. Other examples are the former Defense Special Weapons Agency, which used a risk-assessment model to evaluate force-protection security requirements for terrorist incidents at DOD military bases. The US DOE uses a graded approach to protect its assets based on risk and vulnerability assessments. The Federal Aviation Administration and Federal Bureau of Investigation conduct joint threat and vulnerability assessments on high-risk US airports. Several private companies under contract to government agencies use formal risk-assessment models and methods to identify security requirements. The purpose of this paper is to survey these methods and present an overview of all potential types of sabotage at nuclear power plants. The paper discusses emerging threats and current methods of choice for sabotage--especially vehicle bombs and chemical attacks. Potential consequences of sabotage acts, including economic and political; not just those that may result in unacceptable radiological exposure to the public, are also discussed. Applicability of risk-assessment methods and mitigation techniques are also presented.

The vulnerability analysis methodology developed for fixed nuclear material sites has proven to be extremely effective in assessing associated transportation issues. The basic methods and techniques used are directly applicable to conducting a transportation vulnerability analysis. The purpose of this paper is to illustrate that the same physical protection elements (detection, delay, and response) are present, although the response force plays a dominant role in preventing the theft or sabotage of material. Transportation systems are continuously exposed to the general public whereas the fixed site location by its very nature restricts general public access.

To date, the Department of Energy's (DOE) Material Protection, Control, and Accountancy (MPC and A) program has assisted in the implementation of operational site-wide MPC and A systems at several nuclear facilities in Russia. Eleven sites from the civilian sector have completed the site-wide installations and two have completed sub-site installations. By the end of 1999, several additional sites will have completed site-wide and sub-site system installations through DOE assistance. the effort at the completed sites has focused primarily on the design, integration, and installation of upgraded MPC and A systems. In most cases, little work has been performed to ensure that the installed systems will be sustained. Because of concerns that the installed systems would not be operated in the future, DOE established a sustainability pilot program involving the 11 sites. The purpose of DOE's MPC and A Sustainability Program is to ensure that MPC and A upgrades installed at sites in Russia are effective and will continue to operate over the long term. The program mission is to work with sites where rapid upgrades have been completed to cultivate enduring and consistent MPC and A practices. The program attempts to assist the Russian sites to develop MPC and A organizations that will operate, maintain, and continue to improve the systems and procedures. Future assistance will strive to understand and incorporate culturally sensitive approaches so that the sites take ownership for all MPC and A matters. This paper describes the efforts of the sustainability program to date.

This work has been performed as part of the search for possible ways to utilize the capabilities of laser and particle beams techniques in shock wave and equation of state physics. The peculiarity of these techniques is that we have to deal with micron-thick targets and not well reproducible incident shock wave parameters, so all measurements should be of a high resolution and be done in one shot. Besides the Hugoniots, the experimental basis for creating the equations of state includes isentropes corresponding to unloading of shock-compressed matter. Experimental isentrope data are most important in the region of vaporization. With guns or explosive facilities, the unloading isentrope is recovered from a series of experiments where the shock wave parameters in plates of standard low-impedance materials placed behind the sample are measured [1,2]. The specific internal energy and specific volume are calculated from the measured p(u) release curve which corresponds to the Riemann integral. This way is not quite suitable for experiments with beam techniques where the incident shock waves are not well reproducible. The thick foil method [3] provides a few experimental points on the isentrope in one shot. When a higher shock impedance foil is placed on the surface of the material studied, the release phase occurs by steps, whose durations correspond to that for the shock wave to go back and forth in the foil. The velocity during the different steps, connected with the knowledge of the Hugoniot of the foil, allows us to determine a few points on the isentropic unloading curve. However, the method becomes insensitive when the low pressure range of vaporization is reached in the course of the unloading. The isentrope in this region can be measured by recording the smooth acceleration of a thin witness plate foil. With the mass of the foil known, measurements of the foil acceleration will give us the vapor pressure.

The Autoridad Regulatoria Nuclear of Argentina (ARN), the International Atomic Energy Agency (IAEA), ABACC, the US Department of Energy, and the US Support Program POTAS, cooperated in the development of a Remote Monitoring System for nuclear nonproliferation efforts. This system was installed at the Embalse Nuclear Power Station last year to evaluate the feasibility of using radiation sensors in monitoring the transfer of spent fuel from the spent fuel pond to dry storage. The key element in this process is to maintain continuity of knowledge throughout the entire transfer process. This project evaluated the fundamental design and implementation of the Remote Monitoring System in its application to regional and international safeguard efficiency. New technology has been developed to enhance the design of the system to include storage capability on board sensor platforms. This evaluation has led to design enhancements that will assure that no data loss will occur during loss of RF transmission of the sensors.

J. P. Wilcoxon and G. A. Samara Crystalline, size-selected Si nanocrystals in the size range 1.8-10 nm grown in inverse micellar cages exhibit highly structured optical absorption and photoluminescence (PL) across the visible range of the spectrum. The most intense PL for the smallest nanocrystals produced This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, make any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. to induce a useful level of visible photoluminescence (PL) from silicon (Si). The approaches understood. Visible PL has been observed from Si nanocrystals, or quantum dots, produced by a variety of techniques including aerosols,2 colloids,3 and ion implantation.4 However, all of The optical absorption spectra of our nanocrystals are much richer in spectral features spectrum of bulk Si where the spectral features reflect the details of the band structure shown in nanocrystals estimated to have a Si core diameter of 1-2 nm. These measured quantum those in the spectrum of bulk Si in Fig. 1 are striking indicating that nanocrystals of this size 8-Room temperature PL results on an HPLC size-selected, purified 2 nm nanocrystals but blue shifted by -0.4 eV due to quantum confinement. Excitation at 245 nm yields the PL shows the PL spectrum for a similar sample excited at 490 nm (2.53 eV) trapped excitons at the surface of Si nanocrystals. The excitons are obtained for dimer bonds 1.8- 10 nm. These nanocrystals retain bulk-like optical absorption and an indirect bandgap Figure 1. The absorption spectrum of d = 2 nm Si nanocrystals compared to that of bulk7 Si. Figure 2. The extinction and PL (excitation at 490 nm) spectra ford= 8-10 nm Si nanocrystals.

Multiple-energy (30-325 keV) O{sup +} implantation into GaN field-effect transistor structures (n {approximately} 10{sup 18} cm{sup {minus}3}, 3000 {angstrom} thick) can produce as-implanted sheet resistances of 4 x 10{sup 12} {Omega}/{open_square}, provided care is taken to ensure compensation of the region up to the projected range of the lowest energy implant. The sheet resistance remains above 10{sup 7} {Omega}/{open_square} to annealing temperatures of {approximately} 650 C and displays an activation energy of 0.29 eV. No diffusion of the implanted oxygen was observed for anneals up to 800 C.

The thermal oxidation of pentacontane (C{sub 50}H{sub 102}), and of the homopolymer polyisoprene, has been investigated using {sup 17}O NMR spectroscopy. By performing the oxidation using {sup 17}O labeled O{sub 2} gas, it is possible to easily identify degradation products, even at relatively low concentrations. It is demonstrated that details of the degradation mechanism can be obtained from analysis of the {sup 17}O NMR spectra as a function of total oxidation. Pentacontane reveals the widest variety of reaction products, and exhibits changes in the relative product distributions with increasing O{sub 2} consumption. At low levels of oxygen incorporation, peroxides are the major oxidation product, while at later stages of degradation these species are replaced by increasing concentrations of ketones, alcohols, carboxylic acids and esters. Analyzing the product distribution can help in identification of the different free-radical decomposition pathways of hydroperoxides, including recombination, proton abstraction and chain scission, as well as secondary reactions. The {sup 17}O NMR spectra of thermally oxidized polyisoprene reveal fewer degradation functionalities, but exhibit an increased complexity in the type of observed degradation species due to structural features such as unsaturation and methyl branching. Alcohols and ethers formed from hydrogen abstraction and free radical termination.

A new forcefield model was developed for modeling phosphate materials that have many important applications in the electronics and biomedical industries. Molecular dynamics simulations of a series of lithium phosphate glass compositions were performed using the new forcefield model. A high concentration of three member rings (P{sub 3}O{sub 3}) was found in the glass of intermediate composition (0.2 Li{sub 2}O {center_dot} 0.8 P{sub 2}O{sub 5}) that corresponds to the minimum in the glass transition temperature curve for the compositional series.

An eddy-current scanning system is being developed to allow the International Atomic Energy Agency (IAEA) to verify the integrity of nuclear material storage containers. Such a system is necessary to detect attempts to remove material from the containers in facilities where continuous surveillance of the containers is not practical. Initial tests have shown that the eddy-current system is also capable of verifying the identity of each container using the electromagnetic signature of its welds. The DOE-3013 containers proposed for use in some US facilities are made of an austenitic stainless steel alloy, which is nonmagnetic in its normal condition. When the material is cold worked by forming or by local stresses experienced in welding, it loses its austenitic grain structure and its magnetic permeability increases. This change in magnetic permeability can be measured using an eddy-current probe specifically designed for this purpose. Initial tests have shown that variations of magnetic permeability and material conductivity in and around welds can be detected, and form a pattern unique to the container. The changes in conductivity that are present around a mechanically inserted plug can also be detected. Further development of the system is currently underway to adapt the system to verifying the integrity and identity of sealable, tamper-indicating enclosures designed to prevent unauthorized access to measurement equipment used to verify international agreements.

Surface texture promotes enhanced light absorption in Si solar cells. The quality of lower cost multicrystalline-silicon (mc-Si) has increased to the point that its cell performance is close to that of single c-Si cells, with the major difference resulting from the inability to texture mc-Si affordably. This has reduced the cost-per-watt advantage of mc-Si. Surface texturing aimed at enhanced absorption in Si has been historically obtained by creating multimicrometer-sized pyramids using anisotropic wet etchants on single-crystalline silicon that take advantage of its single crystalline orientation. Since the surface feature sizes are several times the length of the incident solar wavelengths involved, the optical analysis of the reflected and absorbed light can be understood using geometrical optics. Geometrical textures reduce reflection and improve absorption by double-bounce and oblique light coupling into the semiconductor. However, geometrical texturing suffers from several disadvantages that limit its effectiveness. Some of these are listed below: (a) Wet-chemical anisotropic etching used to form random pyramids on <100> crystal orientation is not effective in the texturing of low-cost multicrystalline wafers, (b) Anti-reflection films deposited on random features to reduce reflection have a resonant structure limiting their effectiveness to a narrow range of angles and wavelengths. Various forms of surface texturing have been applied to mc-Si in research, including laser-structuring, mechanical grinding, porous-Si etching, and photolithographically defined etching. However, these may be too costly to ever be used in large-scale production. A Japanese firm has reported the development of an RIE process using Cl{sub 2} gas, which textures multiple wafers per batch, making it attractive for mass-production [1]. Using this process, they have produced a 17.1% efficient 225-cm{sup 2} mc-Si cell, which is the highest efficiency mc-Si cell of its size ever reported. This proves that RIE texturing does not cause performance-limiting damage to Si cells. In this paper, we will discuss an RIE texturing process that avoids the use of toxic and corrosive Cl{sub 2} gas.

The safe, secure and reliable application of Microelectromechanical Systems (MEMS) devices requires knowledge about the distribution in material and mechanical properties of the small-scale structures. A new testing program at Sandia is quantifying the strength distribution using polysilicon samples that reflect the dimensions of critical MEMS components. The strength of polysilicon fabricated at Sandia's Microelectronic Development Laboratory was successfully measured using samples 2.5 microns thick, 1.7 microns wide with lengths between 15 and 25 microns. These tensile specimens have a freely moving hub on one end that anchors the sample to the silicon die and allows free rotation. Each sample is loaded in uniaxial tension by pulling laterally with a flat tipped diamond in a computer-controlled Nanoindenter. The stress-strain curve is calculated using the specimen cross section and gage length dimensions verified by measuring against a standard in the SEM.

In this paper, we introduce a new approach for altering the properties of bridged polysilsesquioxane xerogels using post-processing mobilization of the polymeric network. The bridging organic group contains latent functionalities that can be liberated thermally, photochemically, or by chemical means after the gel has been processed to a xerogel. These modifications can produce changes in density, volubility, porosity, and or chemical properties of the material. Since every monomer possesses two latent functional groups, the technique allows for the introduction of high levels of functionality in hybrid organic-inorganic materials. Dialkylenecarbonate-bridged polysilsesquioxane gels were prepared by the sol-gel polymerization of bis(triethoxysilylpropyl)carbonate (1) and bis(triethoxysilylisobutyl)-carbonate (2). Thermal treatment of the resulting non-porous xerogels and aerogels at 300-350 C resulted in quantitative decarboxylation of the dialkylenecarbonate bridging groups to give new hydroxyalkyl and olefinic substituted polysilsesquioxane monolithic xerogels and aerogels that can not be directly prepared through direct sol-gel polymerization of organotrialkoxysilanes.

Sandia National Laboratories has demonstrated significant performance gains in crystalline silicon solar cell technology through the use of plasma-processing for the deposition of silicon nitride by Plasma Enhanced Chemical Vapor Deposition (PECVD), plasma-hydrogenation of the nitride layer, and reactive-ion etching of the silicon surface prior to the deposition to decrease the reflectivity of the surface. One of the major problems of implementing plasma processing into a cell production line is the batch configuration and/or low throughput of the systems currently available. This report describes the concept of a new in-line plasma processing system that could meet the industrial requirements for a high-throughput and cost effective solution for mass production of solar cells.

Surface texturing of Si to enhance absorption particularly in the IR spectral region has been extensively investigated. Previous research chiefly examined approaches based on geometrical optics. These surface textures typically consist of pyramids with dimensions much larger than optical wavelengths. We have investigated a physical optics approach that relies on surface texture features comparable to, or smaller than, the optical wavelengths inside the semiconductor material. Light interaction at this are strongly dependent on incident polarization and surface profile. Nanoscale textures can be tuned for either narrow band, or broad band absorptive behavior. Lowest broadband reflection has been observed for triangular profiles with linewidths significantly less than 100 nm. Si nanostructures have been integrated into large ({approximately}42 cm{sup 2}) area solar cells, Internal quantum efficiency measurements in comparison with polished and conventionally textured cells show lower efficiency in the UV-visible (350-680 mu), but significantly higher IR (700-1200 nm) efficiency.

This paper describes preliminary results in the development of an acoustic wave (SAW) microsensor array. The array is based on a novel configuration that allows for three sensors and a phase reference. Two configurations of the integrated array are discussed: a hybrid multichip-module based on a quartz SAW sensor with GaAs microelectronics and a fully monolithic GaAs-based SAW. Preliminary data are also presented for the use of the integrated SAW array in a gas-phase chemical micro system that incorporates microfabricated sample collectors and concentrators along with gas chromatography (GC) columns.

Chemically sensitive polymers coated on delay lines utilizing shear horizontal surface acoustic wave (SH-SAW) sensors are investigated for the detection of organic analytes in liquid environments. The SH-SAW sensor platform was designed and fabricated on 36{degree} rotated Y-cut LiTaO{sub 3}. By depositing a SiO{sub 2} dielectric layer over the entire device prior to applying the polymer film, partial electrical passivation of the interdigital transducers (IDT) is obtained while increasing the mass sensitivity of the device. Changes in the mechanical properties of the chemically sensitive polymer materials were clearly detectable through a frequency shift at least one order of magnitude larger than that of a coated-quartz crystal resonator (QCR) in a similar experiment.

Low energy electron microscopy (LEEM) and scanning tunneling microscopy (STM) have been used to investigate the faceting of W(111) as induced by Pt. The atomically rough W(111) surface, when fully covered with a monolayer film of Pt and annealed to temperatures higher than {approximately}750 K, experiences a significant morphological restructuring: the initially planar surface undergoes a faceting transition and forms three-sided pyramids with {l_brace}211{r_brace} faces. When Pt is dosed onto the heated surface, the transition from planar to faceted structure proceeds through the nucleation and growth of spatially separated faceted regions, as shown by LEEM. STM reveals the atomic structure of the partially faceted surface, with large planar regions, dotted by clusters of pyramids of various sizes.

The rotorcraft industry is constantly evaluating new types of lightweight composite materials that not only enhance the safety and reliability of rotor components, but also improve performance and extend operating life as well. The tests required for these evaluations are typically quite complex requiring massive test fixtures, in many cases, along with multiple actuators for loading test articles at various points simultaneously. This paper discusses the background for development of the facility, as well as hardware and overall system design and implementation. Additional topics that are covered include data acquisition, implementation of nondestructive inspection techniques during the test process, and some results from the initial test series performed in the facility.

The Accident Response Mobile Manipulator System (ARMMS) is a teleoperated emergency response vehicle that deploys two hydraulic manipulators, five cameras, and an array of sensors to the scene of an incident. It is operated from a remote base station that can be situated up to four kilometers away from the site. Recently, a modular telerobot control architecture called SMART (Sandia's Modular Architecture for Robotic and Teleoperation) was applied to ARMMS to improve the precision, safety, and operability of the manipulators on board. Using SMART, a prototype manipulator control system was developed in a couple of days, and an integrated working system was demonstrated within a couple of months. New capabilities such as camera teleoperation, autonomous tool changeout and dual manipulator control have been incorporated. The final system incorporates twenty-two separate modules and implements eight different behavior modes. This paper describes the integration of SMART into the ARMMS system.

This paper presents a practical approach for integrating automatically designed fixtures with automated assembly planning. Product assembly problems vary widely; here the focus is on assemblies that are characterized by a single base part to which a number of smaller parts and subassemblies are attached. This method starts with three-dimension at CAD descriptions of an assembly whose assembly tasks require a fixture to hold the base part. It then combines algorithms that automatically design assembly pallets to hold the base part with algorithms that automatically generate assembly sequences. The designed fixtures rigidly constrain and locate the part, obey task constraints, are robust to part shape variations, are easy to load, and are economical to produce. The algorithm is guaranteed to find the global optimum solution that satisfies these and other pragmatic conditions. The assembly planner consists of four main elements: a user interface, a constraint system, a search engine, and an animation module. The planner expresses all constraints at a sequencing level, specifying orders and conditions on part mating operations in a number of ways. Fast replanning enables an interactive plan-view-constrain-replan cycle that aids in constrain discovery and documentation. The combined algorithms guarantee that the fixture will hold the base part without interfering with any of the assembly operations. This paper presents an overview of the planners, the integration approach, and the results of the integrated algorithms applied to several practical manufacturing problems. For these problems initial high-quality fixture designs and assembly sequences are generated in a matter of minutes with global optimum solutions identified in just over an hour.

Automatic assembly sequencing and visualization tools are valuable in determining the best assembly sequences, but without Human Factors and Figure Models (HFFMs) it is difficult to evaluate or visualize human interaction. In industry, accelerating technological advances and shorter market windows have forced companies to turn to an agile manufacturing paradigm. This trend has promoted computerized automation of product design and manufacturing processes, such as automated assembly planning. However, all automated assembly planning software tools assume that the individual components fly into their assembled configuration and generate what appear to be perfectly valid operations, but in reality some operations cannot physically be carried out by a human. For example, the use of a ratchet may be reasoned feasible for an assembly operation; however, when a hand is placed on the tool the operation is no longer feasible, perhaps because of inaccessibility, insufficient strength or human interference with assembly components. Similarly, human figure modeling algorithms may indicate that assembly operations are not feasible and consequently force design modifications, however, if they had the capability to quickly generate alternative assembly sequences, they might have identified a feasible solution. To solve this problem, HFFMs must be integrated with automated assembly planning which allows engineers to quickly verify that assembly operations are possible and to see ways to make the designs even better. This paper presents a framework for integrating geometry-based assembly planning algorithms with commercially available human figure modeling software packages. Experimental results to selected applications along with lessons learned are presented.

A molecular-level understanding of mineral-water interactions is critical for the evaluation and prediction of the sorption properties of clay minerals that may be used in various chemical and radioactive waste disposal methods. Molecular models of metal sorption incorporate empirical energy force fields, based on molecular orbital calculations and spectroscopic data, that account for Coulombic, van der Waals attractive, and short-range repulsive energies. The summation of the non-bonded energy terms at equally-spaced grid points surrounding a mineral substrate provides a three dimensional potential energy grid. The energy map can be used to determine the optimal sorption sites of metal ions on the exposed surfaces of the mineral. By using this approach, we have evaluated the crystallographic and compositional control of metal sorption on the surfaces of kaolinite and illite. Estimates of the relative sorption energy and most stable sorption sites are derived based on a rigid ion approximation.